Research progress of electrolytes for aluminum ion batteries
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摘要: 由于社会的快速发展，人们对二次离子电池的要求日益提高。铝离子电池具有成本低、安全性高、循环性能好等优点，是未来替代锂离子电池的理想储能体系。电解质作为电池系统重要组成之一，起到传输离子、连通电路的作用，对电池性能具有直接影响。因此，设计和制备具有良好综合性能的电解质一直是铝离子电池领域的研究热点。本文对目前铝离子电池的液态电解质、无机固态电解质和聚合物电解质的研究现状进行了总结，从成本、电化学窗口、化学稳定性和离子电导率等方面对它们的性能进行了分析，并对未来铝离子电池电解质的发展方向进行了展望。Abstract: Due to the rapid development of society, demands for secondary ion batteries are gradually increasing. Aluminum-ion battery has a lot of advantages, such as low cost, high safety and good cycle performance. Thus, it is an ideal energy storage system to replace lithium-ion battery in the future. As an important component of battery system, electrolyte plays a key role in transferring ions and connecting circuits, and has a direct impact on battery performance. Therefore, designing and preparing of electrolytes with good overall performance has become a research hotspot in aluminum-ion batteries. This article summarizes the current research status of liquid electrolytes, inorganic solid electrolytes and polymer electrolytes for aluminum-ion batteries, analyzes their performance in terms of cost, electrochemical window, chemical stability and ionic conductivity. The future development direction of aluminum-ion battery electrolytes is prospected.
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图 1 铝离子电池使用V2O5纳米线阴极和铝阳极，在三氟甲磺酸铝(Al(OTF)3)溶于体积比为1∶1的碳酸丙烯脂(PC)/四氢呋喃(THF) (a) 和摩尔比为1.1∶1的 AlCl3/1-乙基-3-甲基氯化咪唑盐([EMIM]Cl) (b)中，扫描速率为0.2 mV·s−1时的典型循环伏安图[19]
Figure 1. Typical cyclic voltammograms of Al-ion battery using V2O5 nano-wire cathode and aluminium anode in 1∶1 volume ratio of aluminum trifluoromethanesulfonate (Al(OTF)3) in propylene carbonate/tetrahydrofuran (PC/THF) (a) and 1.1∶1 molar ratio of AlCl3 in 1-ethyl-3-methylimidazolium chloride ([EMIM]Cl) at a sweep rate of 0.2 mV·s−1 (b)[19]
图 2 (a) 世伟洛克型电池中的不同摩尔比(1.1、1.3、1.5 和 1.8)的AlCl3/[EMIM]Cl 离子液体电解质，在电流密度为66 mA·g−1时Al/热解石墨箔(PG)电池的恒电流充放电曲线；(b) 离子液体电解质AlCl3/[EMIM]Cl摩尔比为1.3的拉曼光谱[20]
Figure 2. (a) Galvanostatic charge and discharge curves of Al/pyrolytic graphite (PG) cells at a current density of 66 mA·g−1 in various mole ratios (1.1, 1.3, 1.5 and 1.8) of AlCl3/[EMIM]Cl ionic liquid electrolytes in a Swagelok-type cell; (b) Raman spectrum of the ionic liquid electrolyte with a mole ratio of AlCl3/[EMIM]Cl=1.3[20]
EMI+—1-ethyl-3-methyl-1H-imidazolium+
图 3 (a) 苯的含量与离子电导率和离子液体浓度的关系；(b) 含有不同比例苯的离子液的半电池CV曲线；(c) 对应于图3(b)的阳极和阴极电流密度峰值；(d) 阳极电流密度峰值与半电池CV扫描速率的关系[21]
Figure 3. (a) Concentration and ionic conductivity according to the addition ratio of benzene in ionic liquid; (b) Half-cell CV according to the addition ratio of benzene; (c) Anodic and cathodic current density peaks corresponding to Fig. 3(b); (d) Relationship between anodic current density peak and scan rate of half-cell CV[21]
Ip—Anodic current density peak; C—Electrolyte concentration
图 4 不同离子液体的电化学窗口和电导率的比较：(a) 循环伏安图；(b) 电导率-温度(δ-T)曲线；(c) 离子液体的Arrhenius拟合曲线[24]
Figure 4. Comparison of the electrochemical windows and conductivities of different ionic liquids: (a) Cyclic voltammogram; (b) Conductivity-temperature (δ-T) curves; (c) Arrhenius fitted curves of ionic liquids[24]
δ—Ionic conductivity
图 5 (a) 未处理和处理后铝阳极表面铝沉积/溶解的示意图；(b) 铝箔在0.5 mol/L Al(OTF)3/1-丁基-3-甲基咪唑三氟甲磺酸盐([BMIM]OTF)和AlCl3/[BMIM]Cl=1.1∶1摩尔比中浸泡24 h前后的SEM图像[25]
Figure 5. (a) Schematic diagram of Al deposition/dissolution on surface of untreated and treated Al anode; (b) SEM images of Al foils before and after immersion in 0.5 mol/L Al(OTF)3/1-butyl-3-methylimidazolium trifluoromethanesulfonate ([BMIM]OTF) and AlCl3/[BMIM]Cl=1.1∶1 mole ratio for 24 h[25]
图 7 在摩尔比AlCl3/尿素=1.3电解质中，石墨和铝电极的CV测试：(a) 石墨嵌入/脱嵌(扫速为1 mV·s−1)对应的电池主要充放电曲线；(b) 铝沉积和溶解(扫速为0.5 mV·s−1)使用三电极体系；(c) 使用AlCl3/尿素=1.3摩尔比电解质在100 mA·g−1 (循环20圈)的恒流充放电曲线；(d) 电池充电示意图(Al沉积和阴离子嵌入石墨)[33]
Figure 7. CV of graphite and aluminum electrodes in AlCl3/urea=1.3 electrolyte (by mole): (a) Graphite intercalation/deintercalation (1 mV·s−1), with corresponding major battery charge/discharge curve features indicated; (b) Aluminum deposition and stripping (0.5 mV·s−1) using three aluminum electrode set up; (c) Galvanostatic charge/discharge curve using AlCl3/urea =1.3 electrolyte (by mole) at 100 mA·g−1 (cycles 20); (d) Schematic of battery charging (Al deposition and anion intercalation in graphite)[33]
图 8 基于AlCl3/Et3NHCl摩尔比为1.5的Al-石墨烯(Al-G)电池的电化学性能：(a) 扫速为1 mV·s−1时的循环伏安曲线；(b) 电流密度为5 A·g−1时具有代表性的恒流充放电曲线；(c) 恒流循环
30000 次(电流密度为5 A·g−1，上/下截止电压为2.54 V/0.7 V)[34]Figure 8. Electrochemical performance of the Al-graphene (Al-G) battery based on the AlCl3/Et3NHCl electrolyte at mole ratio of 1.5: (a) Cyclic voltammogram (CV) curve at 1 mV·s−1; (b) Representative galvanostatic charge/discharge curve at 5 A·g−1; (c)
30000 cycles of galvanostatic cycling (Current density at 5 A·g−1 and 2.54 V/0.7 V upper/lower cut-off voltage)[34]
图 9 25℃下AlCl3/三甲胺盐酸盐(TMAHCl)离子电导率与AlCl3/[EMIM]Cl[36]、AlCl3/[BMIM]Cl[37]、AlCl3/三乙胺盐酸盐(TEAHCl)和AlCl3/Urea离子电导率的比较[35]
Figure 9. Comparison of AlCl3/trimethylammonium chloride (TMAHCl) ionic conductivity with that of AlCl3/[EMIM]Cl[36], AlCl3/[BMIM]Cl[37], AlCl3/triethylamine hydrochloride (TEAHCl) and AlCl3/urea at 25℃[35]
图 19 Se/介孔碳(CMK-3)复合阴极在铝硒电池中的恒流充放电测试：((a)~(c)) 100、200和500 mA·g−1的充放电曲线；(d) 阴极在不同电流速率下的循环性能[69]
Figure 19. Galvanostatic charge/discharge measurements of Se/mesoporous carbon (CMK-3) composite cathodes in Al-Se batteries: ((a)-(c)) Charge/discharge profiles at 100, 200 and 500 mA·g−1, respectively; (d) Cycling performances of the cathodes at different current rates[69]
表 1 25℃下不同AlCl3与4–乙基吡啶摩尔比配制的电解质的离子电导率、黏度和密度
Table 1. Ionic conductivity, viscosity, and density values of 4-ethylpyridine-AlCl3 electrolytes with various AlCl3 to 4-ethylpyridine molar ratios measured at 25℃
AlCl3/4-ethylpyridine
molar ratioConductivity/
(mS·cm−1)Viscosity/
(mPa·s)Density/
(g·cm−3)1.1 0.71 17.80 1.209 1.2 0.78 19.62 1.214 1.3 0.89 22.36 1.216 1.4 0.91 23.57 1.217 
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表 2 不同温度下铝离子固态电解质离子电导率
Table 2. Ion-conductivity of Al-ion solid electrolyte at different temperatures
Temperature/℃ Ion-conductivity/(S·cm−1) Al(CF3SO3)3 (AF) AlCl3 (ACL) Al(NO3)3 (ANO) 24 5.50×10−6 2.34×10−6 3.98×10−7 40 6.60×10−6 2.38×10−6 6.16×10−7 50 1.19×10−5 3.01×10−6 9.80×10−7 60 2.79×10−5 4.42×10−6 1.89×10−6 70 1.37×10−4 6.70×10−6 1.90×10−6 80 7.65×10−4 1.76×10−5 4.88×10−5 90 1.43×10−3 3.23×10−5 9.07×10−5 100 1.89×10−3 4.95×10−5 1.88×10−4
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